Abstract.A major fraction of fine particle matter consists of organic carbon (OC) but its origin is still inadequately known. In this study the sources of OC were investigated in the northern European urban environment in Helsinki, Finland. Measurements were carried out over one year and they included both filter (PM 1 ) and online methods. From the filter samples OC, elemental carbon (EC), water-soluble OC (WSOC), levoglucosan and major ions were analyzed. Filter data together with the concentrations of inorganic gases were analyzed by Positive matrix factorization (PMF) in order to find the sources of OC (and WSOC) on an annual as well as on a seasonal basis. In order to study the diurnal variation of sources, OC and EC were measured by a semicontinuous OC/EC analyzer and major ions were determined by a Particle-into-Liquid Sampler coupled to ion chromatographs. According to PMF, OC concentrations were impacted by four sources: biomass combustion, traffic, long-range transport and secondary production. On an annual basis the OC concentration was dominated by secondary organic aerosol (SOA). Its contribution to OC was as high as 64% in summer, which besides anthropogenic sources may also result from the large biogenic volatile organic carbon (VOC) emissions in the boreal region. In winter biomass combustion constituted the largest fraction in OC due to domestic wood combustion for heating purposes. Traffic contributed to OC from 15 to 27%. Regarding the diurnal variation, the contribution from traffic was higher from 08:00 to 18:00 on weekdays than on weekends. The contribution from long-range transport to OC was 24% on average. All four sources also influenced the WSOC concentrations, however, the contribution of SOA was significantly larger for WSOC than OC.
Abstract.The Antarctic near-coastal sub-micrometre aerosol particle features in summer were characterised based on measured data on aerosol hygroscopicity, size distributions, volatility and chemical ion and organic carbon mass concentrations. Hysplit model was used to calculate the history of the air masses to predict the particle origin. Additional measurements of meteorological parameters were utilised. The hygroscopic properties of particles mostly resembled those of marine aerosols. The measurements took place at 130 km from the Southern Ocean, which was the most significant factor affecting the particle properties. This is explained by the lack of additional sources on the continent of Antarctica. The Southern Ocean was thus a likely source of the particles and nucleating and condensing vapours. The particles were very hygroscopic (HGF 1.75 at 90 nm) and very volatile. Most of the sub-100 nm particle volume volatilised below 100 • C. Based on chemical data, particle hygroscopic and volatile properties were explained by a large fraction of non-neutralised sulphuric acid together with organic material. The hygroscopic growth factors assessed from chemical data were similar to measured. Hygroscopicity was higher in dry continental air masses compared with the moist marine air masses. This was explained by the aging of the marine organic species and lower methanesulphonic acid volume fraction together with the changes in the inorganic aerosol chemistry as the aerosol had travelled long time over the continental Antarctica. Special focus wasCorrespondence to: E. Asmi (eija.asmi@fmi.fi) directed in detailed examination of the observed new particle formation events. Indications of the preference of negative over positive ions in nucleation could be detected. However, in a detailed case study, the neutral particles dominated the particle formation process. Freshly nucleated particles had the smallest hygroscopic growth factors, which increased subsequent to particle aging.
Abstract. Four years of continuous aerosol number size distribution measurements from the Arctic Climate Observatory in Tiksi, Russia, are analyzed. Tiksi is located in a region where in situ information on aerosol particle properties has not been previously available. Particle size distributions were measured with a differential mobility particle sizer (in the diameter range of 7–500 nm) and with an aerodynamic particle sizer (in the diameter range of 0.5–10 μm). Source region effects on particle modal features and number, and mass concentrations are presented for different seasons. The monthly median total aerosol number concentration in Tiksi ranges from 184 cm−3 in November to 724 cm−3 in July, with a local maximum in March of 481 cm−3. The total mass concentration has a distinct maximum in February–March of 1.72–2.38 μg m−3 and two minimums in June (0.42 μg m−3) and in September–October (0.36–0.57 μg m−3). These seasonal cycles in number and mass concentrations are related to isolated processes and phenomena such as Arctic haze in early spring, which increases accumulation and coarse-mode numbers, and secondary particle formation in spring and summer, which affects the nucleation and Aitken mode particle concentrations. Secondary particle formation was frequently observed in Tiksi and was shown to be slightly more common in marine, in comparison to continental, air flows. Particle formation rates were the highest in spring, while the particle growth rates peaked in summer. These results suggest two different origins for secondary particles, anthropogenic pollution being the important source in spring and biogenic emissions being significant in summer. The impact of temperature-dependent natural emissions on aerosol and cloud condensation nuclei numbers was significant: the increase in both the particle mass and the CCN (cloud condensation nuclei) number with temperature was found to be higher than in any previous study done over the boreal forest region. In addition to the precursor emissions of biogenic volatile organic compounds, the frequent Siberian forest fires, although far away, are suggested to play a role in Arctic aerosol composition during the warmest months. Five fire events were isolated based on clustering analysis, and the particle mass and cloud condensation nuclei number were shown to be somewhat affected by these events. In addition, during calm and cold months, aerosol concentrations were occasionally increased by local aerosol sources in trapping inversions. These results provide valuable information on interannual cycles and sources of Arctic aerosols.
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